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The addition of coating to the black carbon (BC) enhances its absorption as more light is focused by the coating "lens." The absorption enhancement factor (Eabs) of BC is difficult to quantify due to an inadequate representation of its mixing structure and the interaction with radiation. Here, by tracking the evolution of the fresh BC particles in the ambient, we found a transitional stage of the particle Eabs with the non‐BC‐to‐BC mass ratio (RBC) at ∼2, below which there were insufficient coating materials to encapsulate the BC core and the absorption enhancement was not significant (∼14%). When the RBC >∼ 2, obvious absorption enhancement occurred as the BC cores were fully covered. Secondary inorganic species played the most critical role in the coating materials to enhance the "lensing effect." We suppose the particle‐resolved core‐shell Mie model can be applied in the Eabs prediction for most cases. Plain Language Summary: Black carbon is the dominant light‐absorbing component of atmospheric aerosols, significantly affecting the global climate. In the atmospheric aging process, such as condensation and oxidation, fresh BC is gradually coated. The light absorption of BC is significantly associated with the amount of its coating material since the coating could act as "lens" to refract more light toward the BC core. However, this "lensing effect" for BC particles is poorly quantified, bringing uncertainties when evaluating the aerosol radiative forcing. In this study, we found there was a transitional behavior for the light absorption by BC particles which was related to the particle mixing states. When the non‐BC‐to‐BC mass ratio for particles is larger than 2, the coating materials are insufficient to encapsulate the BC core and cannot act as the coating "lens." Our study provides a step forward in understanding the global radiation effect of BC. Key Points: A transitional stage of the absorption enhancement (Eabs) during the evolution of black carbon (BC) was directly observed in the ambientBy tracking the evolution of fresh BC, the predicted Eabs based on the particle‐resolved model showed consistent transitional stageThe secondary inorganic species acted the most critical role in the coating materials to enhance the absorption of BC‐containing particles [ABSTRACT FROM AUTHOR]

• The BC-containing particles were dominated by BC-nitrate particles (BC N, 52.3%) followed by BC-nitrate-sulfate particles (BC NS, 22.4%). • The enhanced mixing state of BC with nitrate was mainly due to the increase of ambient nitrate mass concentration. • The enhanced mixing state of BC with nitrate reduced the light absorption ability of aged BC particles. Black carbon (BC) plays an important role in air quality and climate change, which is closely associated with its mixing state and chemical compositions. In this work the mixing state of BC-containing single particles was investigated to explore the evolution process of ambient BC particles using a single particle aerosol mass spectrometer (SPAMS) in March 2018 in Zhengzhou, China. The BC-containing particles accounted for 61.4% of total detected ambient single particles and were classified into five types including BC-nitrate (BC-N, 52.3%) as the most abundant species, followed by BC-nitrate-sulfate (BC-NS, 22.4%), BCOC (16.8%), BC-fresh (BC-F, 4.5%) and BC-sulfate particles (BC-S, 4.0%). With enhancement of the ambient nitrate concentration, the relative peak area (RPA) of nitrate in BC-N and BC NS particles both increased, yet only the number fraction (N f) of BC N particles increased while the N f of BC-NS particles decreased, suggesting that the enhanced mixing state of BC with nitrate was mainly due to the increase in the ambient nitrate mass concentration. In addition, the N f of BC-N decreased from 65.3% to 28.4% as the absorbing Ångström exponents (AAE) of eBC increased from 0.75 to 1.45, which indicated the reduction of light absorption ability of aged BC particles with the enhanced formation of BC-N particles. The results of this work indicated a change in the mixing state of BC particles due to the dominance of nitrate in PM 2.5 , which also influenced the optical properties of aged BC particles. [Display omitted] [ABSTRACT FROM AUTHOR]

Black carbon (BC) strongly absorbs solar radiation, contributing to global warming. Absorption enhancement of BC particles is difficult to quantify due to an inadequate representation of their complex morphology and mixing structures, as well as interaction with radiation. Here, we apply a 3D method accounting for detailed BC mixing structures to predict the absorption enhancement of individual BC particles (Eabs) and the total BC particle population (Eabs, bulk). The diverse range of mixing structures in individual BC particles leads to variable Eabs that could hardly be predicted by empirical approximations. We find that the volume proportion of the BC embedded in coating (F) determines Eabs when the particle to BC core diameter ratio (Dp/Dc) is larger than 2.0. Our findings reveal the potential mechanism behind the differences in observed and modeled Eabs, bulk. The framework builds a bridge connecting the microscopic mixing structure of individual BC particle with Eabs, bulk. Plain Language Summary: Absorption by black carbon (BC) in the atmosphere strongly affects radiative balance and global climate. The large discrepancies in observed and modeled BC absorption enhancements raise a hot debate. Through applying a new 3D shape model based on electron microscope observations, we propose a new framework that estimates BC absorption enhancement through accounting for mixing structure diversity in individual particles. Our results reveal that the diverse range of mixing structures in individual particles in ambient air leads to complex absorption enhancement that could hardly be predicted by the empirical approximation. The bulk absorption enhancements based on diverse mixing structures provide an explanation for the globally disparate results from laboratory and field observations. The new framework linking microphysical structures to bulk BC optical properties can be used to improve assessment of climate impact. Key Points: The impact on absorption enhancement by embedded fraction is significantly enhanced when BC particle to core diameter ratio >2.0The embedded fraction and coating thickness in aged BC particles can lead to significant differences in bulk absorption enhancementA new bridge is built to connect the microscopic mixing structure of individual aged BC particles with bulk absorption enhancement of BC [ABSTRACT FROM AUTHOR]

The mixing state of refractory black carbon (rBC) aerosols is regarded as a major uncertainty in climate-forcing assessments. This study measured the size distribution and mixing state of rBC using a single-particle soot photometer in the winter of 2022 at an urban site in Beijing. During the campaign, the mean mass concentration of rBC was 0.79 ± 0.63 μg m−3, much lower than that observed in Beijing in the winter of 2013. The number and mass median diameter of the rBC cores were 97 and 200 nm, respectively. The average relative coating thicknesses (RCT) of rBC-containing particles was 1.45 ± 0.27 and average light absorption enhancement (Eabs) was 1.43 ± 0.22. Similar to Eabs, RCT and secondary inorganic aerosols (SIA), especially nitrate, increased with increasing relative humidity. This suggests that higher SIA mass fraction in aerosol with a higher relative humidity in the environment results in a thicker coating and black carbon ageing, thus enhancing light absorption. RCT and Eabs increased rapidly with the increase of PM 1 loading but increased slowly when the PM 1 mass concentration exceeded 60 μg m−3. This indicates that a further increase in the NR-PM 1 species at high PM loading does not increase the thickness of the coatings; therefore, there is no further increase in Eabs. The effects of the chemical composition of the Eabs obtained using the Lindeman, Merenda, and Gold method showed that nitrate plays a prominent role in the enhancement of light absorption, followed by SOA. The rBC mass concentration exhibited clear day-low and night-high patterns which were influenced by the synergetic effects of the boundary layer and emissions. RCT and Eabs presented similar diurnal variations, peaking in the afternoon, which was consistent with the pattern of SIA. This suggests that the SIA produced via photochemical reactions supports the ageing of black carbon-containing particles, leading to light-absorption enhancement. The back-trajectory analysis showed the highest values of rBC mass concentration, RCT, and Eabs appeared in the S cluster suggested that the rBC-containing particles transported from south Beijing were more aged with a thicker coating. While the rBC-containing particles from northern and northwestern Beijing had lower RCT and Eabs values. • Nitrate is the dominant contributor to the coatings on BC and prominent role in light-absorption enhancement. • RCT and Eabs increased rapidly as PM 1 loading increased, but slowly when the PM 1 mass concentration exceeded 60 μg m−3. • The rBC- containing particles transported from south Beijing are more aged with a thicker coating. • ∼15% of the NR-PM 1 mass was bound to BC particles. [ABSTRACT FROM AUTHOR]

Reducing the uncertainty in aerosol radiative forcing requires a comprehensive understanding of the factors affecting black carbon (BC) light absorption. In this study, the characteristics and influencing factors of light absorption enhancement (E abs) of refractory BC (rBC) were investigated by conducting intensive measurements at an urban site in northwest China during the early summer of 2018. On average, the absorption of rBC was enhanced by 34% as a result of the internal mixing of rBC with other aerosol components. Secondary inorganic aerosols (SIAs) were found to have considerable effects on the E abs of rBC. The E abs showed a robust linear relationship with the bulk nitrate/rBC mass ratio in fine particles, with an increase of 3% per nitrate/rBC ratio unit. A notable increase in E abs from dusk to the next morning was observed, in accordance with the diurnal variations in nitrate and sulfate, indicating the excellent contribution of non-photochemical formation of SIAs to E abs. This fact was further supported by the positive correlation of the nitrate/rBC and sulfate/rBC ratios with relative humidity (RH) rather than photochemical indicators. This study indicates that the aqueous and/or heterogeneous formation of SIAs is likely the dominant aging pathway leading to the high E abs of rBC. • Light absorption enhancement (E abs) of BC by coating was observed in northwest China. • Nitrates and sulfates highly affected the E abs , especially nitrates. • The aqueous and/or heterogeneous formation of nitrates and sulfates played a dominant role in E abs. [ABSTRACT FROM AUTHOR]

Recent studies worldwide have demonstrated that coating on atmospheric black carbon (BC) aerosol enhances its absorption potential. However, studies quantifying the light-absorption enhancement (E abs) of BC are extremely limited over the Indian region. The northwestern Indo-Gangetic Plain (IGP) region witnesses annual episodes of substantial crop-residue burning during the post-monsoon season (PoMS), which has been attracting wide attention due to its impact on regional air quality and aerosol characteristics. Chemical aging of these biomass burning (BB) emissions occurs during its long-range transport across the IGP by the weak westerlies, and such atmospheric processing affects their chemical, optical, and radiative properties over downwind locations. This study examines the impact of atmospheric aging of biomass burning emissions on BC light-absorption enhancement (E abs) using extensive, simultaneous measurements of single particle refractory BC and near-real-time mass spectrometry measurements of non-refractory submicron aerosols from an IGP outflow site. It was observed that organics were the dominant submicron aerosol species, and positive matrix factorization analysis of the organics mass spectra suggested that a large fraction of organics (64%) was secondary in nature. The BC particles in the IGP outflow (mass median diameter ∼ 0.18 ± 0.01 μm) were found to be thickly coated with volume-weighted bulk relative coating thickness in the range of 1.3–1.8. The evolution of biomass-burning organic aerosols (BBOA) indicated the presence of significant amounts of aged BBOA during the PoMS. Further, the oxidation products from the evolution of BB emissions contributed to enhanced coatings (∼ 30–70%) on BC. Mie core-shell theory calculations were then used to assess the changes in BC light absorption characteristics due to the coating of non-refractory mass on its cores. It was found that thick coatings on BC led to significant light-absorption enhancement (E abs) (bulk E abs in the range of 1.14–1.94 at 550 nm, depending on the extent of coating). Increased E abs values of ≥1.8 were seen when the coating on BC exceeded 60% of its core size. The modeled bulk E abs at 550 nm depicted a better association with highly oxidized secondary organic aerosols (SOA) than sulfate among the secondary aerosol species, suggesting an SOA-dominant regime. The present findings suggest that the critical impact of the aging of BC and co-emitted species from widespread BB emissions in the IGP outflow should be considered when evaluating the regional radiative implications. • Evidence for the presence of aged biomass-burning organic aerosols in the IGP outflow. • Aged biomass-burning organic aerosols contributed to enhanced coatings on BC cores. • BC absorption potential is enhanced by a factor > 1.5 due to non-refractory coatings. • A higher fraction of secondary organic aerosols resulted in enhanced absorption. [ABSTRACT FROM AUTHOR]

Atmospheric loading of black carbon aerosols influences air quality and visibility, and their mixing state and aerosol chemistry were sensitive to both emission scenarios and regional transport. In this study, the aerodynamic size-resolved mixing state of refractory black carbon aerosols (rBC) was investigated using a novel tandem system consisting of an aerodynamic aerosol classifier (AAC), a single particle soot photometer (SP2), and single-particle-aerosol mass spectrometry (SPA-MS) during the XXIV Olympic Winter Games (OWG) at an urban site in Beijing. Particles with aerodynamic diameter (D ae) of 200 nm and 300 nm were selected by AAC to focus on the effect of relative differences in morphology on the coating thickness, coating compositions, and optical properties of rBC particles. We found that rBC-containing particles with D ae of 300 nm were characterized by a rBC core with a count median diameter (CMD) of 108 ± 4 nm that typically have regular morphology (χ : m e a n ∼ 1) , higher relative coating thickness (RCT: mean ∼1.9), and strong light absorption enhancement (E abs : mean ∼1.5). The rBC-containing particles with D ae = 200 nm normally had irregular shapes (χ : m e a n ∼ 1.4) and weak E abs (E abs : mean ∼1.37). Classification based on air mass clustering and air pollution level revealed that the coating thickness of rBC particles only exhibited unimodal patterns under clean air conditions and distinct bimodal distributions under heavy pollution conditions, implying multiple origins of rBC particles, even during OWG periods. The coating thickness and E abs of rBC particles were greater when influenced by the higher RH air from east. Furthermore, the chemical compositions of the rBC coating quantitatively determined by SPA-MS were used to estimate the possible origins of the D ae = 300 nm, featured by a thicker coating thickness and stronger light absorption enhancement. Our results showed that rBC particles were primarily mixed with organics, nitrate, and sulfate during the XXIV OWG period. The organic components have a limited role in increasing rBC coatings under polluted conditions, while the alkali metal ions (K and Na) associated with traffic emissions and the secondary inorganic species favor the formation of thick coatings. Higher RH makes limited contributions to rBC mixed with sulfate and organics only (BCOC*_S) and pure BC. The relatively fresh BC could directly mix with organics and sulfate at low RH levels while evolving to mix with nitrate at high RH conditions. In addition to high concentrations of locally emitted precursors and high RH that tend to form thick coatings of nitrate-related rBC aerosols, secondary transport from the west and southwest also contributes to rBC aerosols mixed with nitrate with relatively thick coatings. • rBC with an aerodynamic diameter (D ae) of 300 nm typically have regular morphology. • rBC of regular shape(D ae = 300 nm)has thicker coatings and stronger absorption enhancement. • During the OWG, rBC particles were primarily mixed with organics, nitrate and sulfate. • rBC particles had multiple sources, even in the OWG periods. • The organic components have a limited role in increasing rBC coatings under polluted conditions. [ABSTRACT FROM AUTHOR]

The mixing state of black carbon aerosols (BC) has the largest uncertainty for climate forcing evaluation. In this study, a tandem observation, combining a centrifugal particle mass analyzer (CPMA) and a single particle soot photometer (SP2), was conducted to investigate the mixing state of BC in a coastal city in eastern China. First, particles with specific masses (1.0 fg, 2.1 fg, 4.5 fg, 9.7 fg, and 20.1 fg) were selected using CPMA and consecutively measured by SP2 to determine the corresponding BC mass (M BC) of the particle. The mass ratio (M R) of the coating matter to the BC core was used to indicate the coating thickness and aging degree of BC. The results showed that the M R value obtained from the CPMA-SP2 system was well correlated with the mixing state condition derived from the traditional lag-time method. However, the lag-time method tends to misclassify thickly to thinly coated BC as particles with larger masses. The M R generally increased as the mass of BC-containing particles increased. M R showed a clear diurnal pattern with a minimum at 8:00 and a maximum at 13:00 due to photochemical process during the daytime. The larger BC-containing particles had a much weaker diurnal pattern because other secondary processes may contribute more to the coatings for large BC-containing particles. The M R maintained a high value when the air mass was stagnant in the local area with high pollutant concentrations and high relative humidity (RH), while the M R was at its lowest value when the air mass was derived from the marine area with high RH and low pollutant concentrations. These observations suggest that the increase in M R is the result of the combined effect of high RH and high pollutant concentrations. [Display omitted] • Traditional lag-time method tends to misclassify thickly to thinly coated BC as particles with larger masses. • The increase of BC's coating needs the joint action of pollutants precursors, aging time and humidity. • The coating thickness of BC with larger masses had weaker diurnal pattern. [ABSTRACT FROM AUTHOR]